@article{hu_liu_alexy_mandal_bocian_holten_lindsey_2016, title={Panchromatic chromophore–tetrapyrrole light-harvesting arrays constructed from Bodipy, perylene, terrylene, porphyrin, chlorin, and bacteriochlorin building blocks}, volume={40}, ISSN={1144-0546 1369-9261}, url={http://dx.doi.org/10.1039/C6NJ01782G}, DOI={10.1039/c6nj01782g}, abstractNote={Five new chromophore–tetrapyrrole arrays bearing an ethynyl linker have been synthesized to explore the effects of chromophore nature and tetrapyrrole attachment site on panchromatic spectral properties.}, number={9}, journal={New Journal of Chemistry}, publisher={Royal Society of Chemistry (RSC)}, author={Hu, Gongfang and Liu, Rui and Alexy, Eric J. and Mandal, Amit Kumar and Bocian, David F. and Holten, Dewey and Lindsey, Jonathan S.}, year={2016}, pages={8032–8052} } @article{amanpour_hu_alexy_mandal_kang_yuen_diers_bocian_lindsey_holten_2016, title={Tuning the Electronic Structure and Properties of Perylene-Porphyrin-Perylene Panchromatic Absorbers}, volume={120}, ISSN={["1089-5639"]}, DOI={10.1021/acs.jpca.6b06857}, abstractNote={Light-harvesting architectures that afford strong absorption across the near-ultraviolet to near-infrared region, namely, panchromatic absorptivity, are potentially valuable for capturing the broad spectral distribution of sunlight. One previously reported triad consisting of two perylene monoimides strongly coupled to a free base porphyrin via ethyne linkers (FbT) shows panchromatic absorption together with a porphyrin-like S1 excited state albeit at lower energy than that of a typical monomeric porphyrin. Here, two new porphyrin-bis(perylene) triads have been prepared wherein the porphyrin bears two pentafluorophenyl substituents. The porphyrin is in the free base (FbT-F) or zinc chelate (ZnT-F) forms. The zinc chelate (ZnT) of the original triad bearing nonfluorinated aryl rings also was prepared. The triads were characterized using static and time-resolved optical spectroscopy. The results were analyzed with the aid of molecular-orbital characteristics obtained using density functional theory calculations. Of the four triads, FbT is the most panchromatic in affording the most even distribution of absorption spectral intensity as well as exhibiting the largest wavelength span (380-750 nm). The triads exhibit fluorescence yields (0.35 for FbT-F in toluene) that are substantially greater than for the porphyrin benchmarks (0.049 for FbP-F). The singlet excited-state lifetimes (τS) for the triads in toluene decrease in the order FbT-F (2.7 ns) > FbT (2.0 ns) > ZnT (1.2 ns) ∼ ZnT-F (1.1 ns). The τS values in benzonitrile are FbT (1.3 ns) > FbT-F (1.2 ns) > ZnT-F (0.6 ns) > ZnT (0.2 ns). Thus, the free base triads exhibit relatively long (1.2-2.7 ns) excited-state lifetimes in both polar and nonpolar media. The combined photophysical characteristics indicate that FbT and FbT-F are the best choices for panchromatic light-harvesting systems. Collectively, the findings afford insights into the effects of electronic structure on the panchromatic behavior of ethynyl-linked porphyrin-perylene architectures that can help guide next-generation designs and utilization of these systems.}, number={38}, journal={JOURNAL OF PHYSICAL CHEMISTRY A}, author={Amanpour, Javad and Hu, Gongfang and Alexy, Eric J. and Mandal, Amit Kumar and Kang, Hyun Suk and Yuen, Jonathan M. and Diers, James R. and Bocian, David F. and Lindsey, Jonathan S. and Holten, Dewey}, year={2016}, month={Sep}, pages={7434–7450} } @article{alexy_hintz_hughes_taniguchi_lindsey_2015, title={Paley's watchmaker analogy and prebiotic synthetic chemistry in surfactant assemblies. Formaldehyde scavenging by pyrroles leading to porphyrins as a case study}, volume={13}, ISSN={["1477-0539"]}, url={http://www.scopus.com/inward/record.url?eid=2-s2.0-84942899459&partnerID=MN8TOARS}, DOI={10.1039/c5ob01409c}, abstractNote={Facile exchange of micromolar dialkylpyrrolic constituents among a Poisson distribution of aqueous micelles overcomes immense statistical odds against reaction.}, number={39}, journal={ORGANIC & BIOMOLECULAR CHEMISTRY}, publisher={Royal Society of Chemistry (RSC)}, author={Alexy, Eric J. and Hintz, Carl W. and Hughes, Hubert M. and Taniguchi, Masahiko and Lindsey, Jonathan S.}, year={2015}, pages={10025–10031} } @article{alexy_yuen_chandrashaker_diers_kirmaier_bocian_holten_lindsey_2014, title={Panchromatic absorbers for solar light-harvesting}, volume={50}, ISSN={["1364-548X"]}, DOI={10.1039/c4cc06853j}, abstractNote={A set of panchromatic absorbers exhibiting long excited-state lifetimes in both polar and nonpolar media has been prepared. The architectures are based on a porphyrin strongly coupled electronically to 1-4 perylene-monoimides via ethyne linkers. The constructs should find utility in molecular solar-conversion systems.}, number={93}, journal={CHEMICAL COMMUNICATIONS}, author={Alexy, Eric J. and Yuen, Jonathan M. and Chandrashaker, Vanampally and Diers, James R. and Kirmaier, Christine and Bocian, David F. and Holten, Dewey and Lindsey, Jonathan S.}, year={2014}, pages={14512–14515} }